Scalable Polyimide-Organosilicate Hybrid Films for High-Temperature Capacitive Energy Storage.
basic_science · Level V
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- Record sourced from PubMed, PMID 36894169.
- Also identified by DOI 10.1002/adma.202211487.
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Abstract
High-temperature polymer dielectrics have broad application prospects in next-generation microelectronics and electrical power systems. However, the capacitive energy densities of dielectric polymers at elevated temperatures are severely limited by carrier excitation and transport. Herein, a molecular engineering strategy is presented to regulate the bulk-limited conduction in the polymer by bonding amino polyhedral oligomeric silsesquioxane (NH<sub>2</sub> -POSS) with the chain ends of polyimide (PI). Experimental studies and density functional theory (DFT) calculations demonstrate that the terminal group NH<sub>2</sub> -POSS with a wide-bandgap of E<sub>g</sub> ≈ 6.6 eV increases the band energy levels of the PI and induces the formation of local deep traps in the hybrid films, which significantly restrains carrier transport. At 200 °C, the hybrid film exhibits concurrently an ultrahigh discharged energy density of 3.45 J cm<sup>-3</sup> and a high gravimetric energy density of 2.74 J g<sup>-1</sup> , with the charge-discharge efficiency >90%, far exceeding those achieved in the dielectric polymers and nearly all other polymer nanocomposites. Moreover, the NH<sub>2</sub> -POSS terminated PI film exhibits excellent charge-discharge cyclability (>50000) and power density (0.39 MW cm<sup>-3</sup> ) at 200 °C, making it a promising candidate for high-temperature high-energy-density capacitors. This work represents a novel strategy to scalable polymer dielectrics with superior capacitive performance operating in harsh environments.